Coherent anti-Stokes Raman scattering (CARS) spectroscopy is a non-linear optical technique for obtaining Raman spectral information without interference from sample fluorescence. The signal measured in a CARS experiment is on the order of 10 to the 8th power larger than that observed in a conventional laser Raman experiment. The objective of this proposed research is the application of a Nd:YAG unstable resonator laser system to investigate the capability of resonance enhanced CARS as a technique for structural studies of biopolymers. Particular emphasis will be placed on reference arm techniques for removing noise due to laser pulse-to-pulse fluctuations. The relationship between resonance CARS excitation profiles and vibronic spectroscopy will be investigated. The resonance CARS spectra of tryptophan will be determined for a variety of proteins. CARS spectroscopy of highly scattering samples will be attempted with emphasis on the determination of polymerization ratios. The major emphasis will be placed on the demonstration of the phenomenon of chirooptical CARS (Circular Intensity Differential CARS) and its resonance enhanced analog. This technique promises to be a useful method for stereochemical determinations and conformational studies. Exploratory studies of the resonance CARS spectra of enzyme cofactors PLP, DPN and FAD are also proposed.